Apparatus for diffusing gases



June 23, 1936 G. BENNETT 2,045,379

APPARATUS FOR DIFFUSINGGASES Filed Sept, 23, 1952 H mm 1 20 I I a9 22 INVENTOR 11: 7 am 5? 62M wamsssES 26 f2 46 9 0'7 Patented June 23, 1936 I D .STATES PATENT OFFICE;

. 2,045,379 APPARATUS FOB DIFFUSING GASES Owen G. Bennett, Baltimore, Md, asslgnor to Ca alyst Corporation, Baltimore,

Research Mdu a corporation of Maryland Application September 23, 1932, Serial No. 634572 z cum. (01. 13-51) ences in density'of the gases'used, it must be a This invention relates to diffusion of gases, and it is among its objects to provide a simple and eflective apparatus for diffusion of gases, for

' rapid, accurate and readydetermination of various information pertaining to such gases, such as the composition oigaseous mixtures, fractionation or gaseous mixtures in separate one or more constituents, or'determination of the relative density of a gas. A special object is to pro-, vide a diaphragm for use in diflusion apparatus, which is strong and especially suited ior'such purposes. 1

In accordance withknown physical lawsthe velocity at which a. gas diffuses-through a porous, or permeable; diaphragm is inversely proportional to the square root of the density of the gas. Accordingly, if two gases 01' different density are brought into contact with-opposite sides oi a porous diaphragm they-will through it at diiferent rates, and the ratio or their rates of diilusion will be determined by the square root of the inverse ratio of theirv relative densities. If the rates of diifusion could be measured this would provide a means of determining the densityoi a gas, by ascertaining its rate of diilusion in comparison to that of a gas 01' known-density. Thus the-known gas may be enclosed in a space sealed. by a suitable diaphragm and provided with means for measuring pressure and the unknown get passed over the other side 01' the diaphragm. If there is a difl'erence in density between the twogases there will be a difierence in the rate of difiusion through the diaphragm,

'which' will manifest itself by a change in pressure w'ithin the space enclosing the known gas. For example, if air is'enclosed in a chamber having a'porous diaphragm constituting one wall,

and hydrognis passed over the outer surface of the diaphragm, the hydrogen will diil'use through the diaphragm at a greater r'ate'than the air will diffuse outwardly, and the pressure within the cell will increase, This pressure change may be used'to calculate the density 01' the unknown to other ends. For instance, the various constituent's of a gaseous mixture will ilnd their way through the pores of. the diaphragm independently of the others, which renders it applicable to analysis of gaseous mixtures, and to separation of constituents from a gaseous mixture.

Certain essential features must be embodied in the practical and satisfactory appllcation'of these principles. For instance'the device must give a large pressure difference for small diilerable-for this purpose, being either delicate, tedious and'slow in use, or requiring skilled attention, or having unsatisfactory diaphragms.

The invention may be described in connection with the accompanying drawingfin which Fig. 1 is a central sectional view through one apparatus embodying the invention; Fig. 2 a View simi-- lar-to Fig. 1 through a modified form of apparatus; and Figs. 3 and 4 sectional views taken on lines III-IIIand IV-IV, respectively, Fig. 2.

The invention is predicated in part upon my discovery that for satisfactory compliance with the requirements of such an apparatus it'is necessary to passthe unknown gas, i. e. thegas'under investigation, over the surface or the permeable diaphragm at a rate sufiiciently high that the compositionof the unknown gas will not. be Inaterially changed by the clifiusionprocess, i. e.

predicated further on my discovery that it isnec essary in a satisfactory and practicable apparatus that the volume of the known, or standard, gas be small compared with the area of the diaphragm, i; e. the ratio of the diaphragmarea to the volume of standard gas must be large. I have discovered also, and this is a particularly important feature of the invention, that especially desirable' results attend the use of. diaphragms compressed from metallic nickel prepared in a state of exceedingly fine subdivision by amalgamation of nickel with mercury and vacuum distillation of the mercury fromthe amalgam, as will be described more fully hereinafter.

The invention may be described morein detail in connection with the accompanying drawing. Having reference to Fig. 1-, the apparatus shown comprises a hollow casing i defining an internalchamber closed at one end, e. g. by a base portion 2 integral therewith. The upper end of thecasing is closed by a removable head, that shown comprising a plug member 3 provided at its lower end with anoutwardly projecting flange 4 which'is engagedby a compression sleeve 5 threaded exteriorly to engage cooperating threads 55 6 formed in the opening in casing l. Flange 4 is pressed by compression sleeve 5 against a ring member 1 seated on an internal flange Ia. This ring carries a diaphragm 8, permeable by gas, which divides the chamber within the easing into two separated spaces 9 and ID. The diaphragm ring 1 should make a gas tight fit with flange 1a and plug 3, and gaskets may be used if need be.

Space 9 acts as an enclosing chamber for confining the gas used as a standard in the practice of the invention. This gas may be introduced into the chamber by any example through a valve H which opens into space 9, a similar valve l2 being provided for sweeping out the space before and after the apparatus is used. The gas to be investigated, i. e. the unknown gas, is flowed through space III in contact with the outer side of diaphragm.8.. In the embodiment shown the unknown gas is introduced through a valve IS in plug 3 which opens into a duct [4 bored longitudinally through the plug- The gas flows intospace l0 over the upper surface of diaphragm- 8 in intimate contact therewith, and then passes into an annular channel IS in the bottom of the plug, and escapes thence through a duct '16 to an outflow tube H. The plug may also be provided with a valve l8 opening into duct M, for a purpose presently to be described. A pressure-measuring means, not shown, is connected to space 9, as by a nipple l9. Such pressure-indicating means are well known in the art.

An .important in causing the unknown gas to move at a relativelyhigh velocity over the suriace of the diaphragm. This may be accomplished, as shown in Fig. 1, by making space In relatively narrow, i. e. so that the'conduit which is formed between the diaphragm and the closure plug is narrow. This causes the gas to move over the diaphragm at high velocity. My work has shown that this is necessary to obtain accurate results in the use of the apparatus, provided by this invention, it being necessary to move themknown gas over the diaphragm at a rate such that diffusion from or into the unknown gas does not materially alter its composition. By moving the'unknown gas at relatively high velocity such diffusion as takes place is negligible as regards composition change, and can be considered constant.

creased indefinitely,

I have discovered further that in order rapidly to attain equilibrium conditions it is necessary also to proportion the volume of known gas with respect to the area of the diaphragm. For example, using the same diaphragm and the same gases, the. rate oi. diffusion will be the same irrespective of the volume of the enclosed standard gas. However, the maximum pressure change due to the diffusion will be attained more slowly the greater the volume of the standard gas. In accordance with this invention, the volume of standard gas is made small compared with the area of the diaphragm, whereby rapidly to obtain the maximum pressure change due to the difiusion. For the attainment of the most accurate results, however, the ratio of volume of known gas to the diaphragm area cannot be inbecause with the pressureindicating means now available a change in volume'due to the actuation of the gauge or manometer or other means occurs as the gas pressure changes. Thus as the pressure. within the space is increased, the resultant actuation of'the indicating device will increase suitable means, for

feature of this invention resides creasing the exposed diaphragm area.

the volume or the space. If the volume of gas is very small, such volume changes due to the indicating means will represent a substantial proportion of the initial gas volume, and will therefore cause erroneous results. Thusalthough for the reason previously stated the ratio of the diaphragm area to the volume of the gas enclosing space should be large, due regard should be given to the ratio of that volume to. the change in volume caused by actuation of the gauge or the like, to minimize error. This latter factor will vary according to the particular type of means used, but its effect will be readily obtainable for each such means and proposed size of known gas enclosing space.

In accordance with the principles just stated, I have found that for many purposes the gas enclosing space should not be smaller than that which would be changed more than 20 per cent by actuation of the pressure measuring device, and it should not exceed four units of volume per unit oi. diaphragm area.

As an illustration of the application of these factors, satisfactory results were obtained with an apparatus such as shown in Fig; 1 having a diaphragm 1-inch in diameter disposed approximately one-half inch" from the bottom 2 of the casing. This diaphragm positioning formed a space 9, for known gas, of approximately 0.36 cubic inch volume. The bottom of plug 3 was disposed approximately phragm. With this apparatus, andusing a rate of flow of unknown gas of about one liter per minute satisfactory readings were obtained using a Bourdon-type pressure gage, equilibrium being reached in about 35 to 40 seconds.

In the use of this apparatus for determination of the density of a gas, valves H and I2 are opened, and space 9 is swept out with the known, or standard, gas, supplied, for example, through valve ll. Dry air is the most economical and desirable gas for this purpose, particularly since gas densities are generallycalculated with respect to air. Atthe same time space I is swept out with the standard gas supplied through valve l8. Valve I3, connected to a source oi! the gas to be tested (unknown gas), is closed during this inch above the diaoperation. When the two spaces have been thorthe pressure in space 9 willincrease or decrease,

depending upon whether diffusion takes place more rapidly; into ,or from the knowngas. The pressure developed at equilibrium can be used to calculate the density of the unknown gas.

- Although in the apparatus shown inFig. 1 space 8, which encloses the standard gas, cannot be reduced in volume indefinitely for the reason explained hereinabove, the rate at which equilibrium-is obtained may be increased, without decreasing the accuracy of the result, by in- This does not introduce the source of error referred to previously. This may be done most suitably by the use of a plurality of diaphragms, for instance, a pair oi' diaphragms constituting opposite walls oi the standard gasenclosing space. Such an apparatus is shown in Figs. 2 to 4. This embodiment comprises a tubular casing to pro- 75 conduit in various ways. One advantageous con-' collar 2|, and against each side of the collar there is pressed a ring la carrying a diaphragm 8a, as in the preceding embodiment. These rings are pressed firmly through disc members 22 by means-of compression plugs 23 threadably engaging at 2| in the ends of the casing. The

space between the discs 8a thus forms a stand-' ard gas enclosing space 9a, Fig. 2. As in the apparatus of Fig. 1, rings la should seat tightly; preferably they are accurately ground to collar 2! and discs 22 to this end. Space 9a is connected by a nipple 25 to a suitable pressure indicating device, not shown. Standard gas is introduced into space 9a through a valve 26 and a bore 21 extending through the casing into space 90.. A valve 28 similarly connected to space 9a provides for sweeping out the chamber with standard gas, as described hereinabove.

By reason of the fact that the diaphragm is offset in ring 1a from its surfaces it formswith disc 22, a. conduit Illa, Fig. 2, for passage of unknown gas over the exterior of the diaphragm.

This construction gives the restricted passage needed to cause the gas to move at high velocity. The unknown gas may be flowed through this struction is that shown in Figs. 2 to 4. A groove 28 disposed peripherally in the edge of disc 22 is connected by a series of radial bores 30 to an annular internal groove 3! facing' toward the exterior of disc 8a. Disposed centrally of the disc is a transverse bore 32 aligned with a similar bore 33 formed in plug 23, forming means for outflow of gas from space |a. Unknown gas is led to discs 22 through a valve 3 to a bore 35 formed longitudinally in the casing. This bore has side branches 35a which are positioned to align exactly with groove 29 of disc 22. The unknown gas thus flows through valve '34, duct 35, intoegroove 29, and thence through bores 30 into'gro'ove-il, from whence it flows over the outer surface of disc 8a, and escapes through bores 32 and 33. A valve 36 arranged similarly to valve 34 may be provided for introducing standard as, e. g., air, to sweep out unknown gas remaining in the apparatus-as in the caseof Fig. 1.

No detailed description of the use of this apparatus rieed be given, its use being wholly similar to that of Fig. 1. However, as illustrating the benefits in speed of operation, as compared with Fig. 1, it may be noted that using air as the standard gas, and hydrogen as the unknown gas =(l liter per minute), and using the diajphragm presently to be described, an equilibrium pressure of 150 inches of water was developed in' 15 seconds. With a diaphragm of the same size and material, and the same volume of air, with' other operating conditionsidentical, the appara tus shown in Fig. 1, required about 37 seconds to develop the same pressure.

A particular feature of. the invention resides in the use of diaphragms of a novel character. I have found that especially bene'flcialresults are obtained by the use of diaphragr'ns made by compressing metallic nickel in a state of exceedingly fine subdivision. The most suitable metal- I 1 lie nickel for this purpose is prepared by a special procedure, according to which there is formed a nickel amalgam, and the mercury is distilled therefrom under high vacuum and in theabsence of gases which react with the nickel.

The nickel remains as an impalpable powder of .75.

exceptionally fine particle size. The unique charuseful for analytical purposes, and for separation ment. that, within the scope of the appended claims,

the invention may be practiced otherwise than acter of the nickel powder thus produced is evidenced by the fact that it unites under presj I sure, without the use of heat or binders, to form coherent bodies having the appearance of massive nickel. V V I This material may be compressed to form a strong and coherent body suitable for use in the" For example, diatheir pores are so fine that gases pass through themonly by true diffusion, because they are strong, give rapid readings, and because among other things, substantial pressures can bebuilt up with them.

The invention is applicable to purposes other than density determinations, as will be understood by those skilled in the art. Thus, the rapidity of equilibrium attainment renders it of gaseous mixtures. The sturdiness, rapidity of action, and substantial pressures which can be built up are advantageous for the foregoing purposes, as well as making-other applications feasible, including its use as a detector element in alarm apparatus for use in signalling abnormal conditions in gas atmosperes, such as the signalling of the presence of dangerous amounts of explosive gases in mine atmospheres, and other similar applications.

Since the density of a gas or the presence of a particular constituent in a gaseous mixture determines the characteristics of those materials, the term "quantitatively determining a characteristic of a gas is used in the claims to concisely include reference to the treatment of a gas for analyzing it with referenceto one or more constituents, or to determine its density.

invention and have illustrated and described what I now consider to represent. its best embodi- However, I desire to have it understood as specifically illustrated and described.

I claim: l'. Anapparatus for diffusion of gases comprising a hollow casing closed at its ends, a pair of permeable diaphragms mounted in spaced relation in said casing and forming therebetween a gas-enclosing space, means for introducing and confining a gas in said space, means forming with the exterior of each of said-diaphragms a separate gas conduit of width restricted to cause gas passed therethrough to move at high velocity over the surface of the diaphragm exteriorly of said chamber, means for supplying gas to said conduits, and pressure-responsive means associated with said gas-enclosing space to indicate the pressure of gas confined therein. I 2. As anew article'of manufacture, a gas diffusion diaphragm composed of finely divided nickel compressed into a strong and coherent body, the nickel having been formed by evaporation of mercury from a mercury-nickel amalgam to leave the nickel in a state of exceedingly fine sub-division.

- OWEN G. BENNETT. 

